Abstract
The coupling between ionic and electronic species and their dynamic interplay lay the foundation for organic electrochemical transistors (OECTs) to transduce and amplify bio(chemical) signals through ion-modulated conductivity. However, the operation of most reported OECTs is typically dominated by single ions, e.g. anions for p-type accumulation devices, mainly due to the challenge of regulating ion dynamics to enable both types of ions to play a role during the electrochemical doping process. In this study, we propose that electrochemical doping of an OECT channel can occur via an anion-cation dual-doping mechanism, where cation expulsion and anion injection occur simultaneously. By designing a p-type organic mixed ionic-electronic conductor, Pu2gT, with strong side chain-cation interactions, we successfully decelerate the cation transport dynamics, allowing the dual-doping process to occur. As a result, Pu2gT OECT exhibits improved current sensitivity compared with the anion-dominated counterpart, showing potential in high-quality electrocardiogram signal acquisition and ion concentration discrimination. Furthermore, incorporating crown ether additives into Pu2gT enhances the dual-doping effect by further delaying cation dynamics, leading to even higher device performance. This dual-doping mechanism deepens the understanding of OECT working principles and opens avenues for achieving state-of-the-art bioelectronic devices.
Acknowledgments
The authors thank Dr. Eric Schaible and Dr. Chenhui Zhu at beamline 7.3.3 for assistance in data acquisition. The authors further acknowledge Biolin Scientific AB for help in EQCM-D experiments and data analysis, as well as the Instrument Analysis Center of Xi’an Jiaotong University for their assistance in cryo-EM experiments.
Funding
This work was supported by the National Key Research and Development Program of China (2024YFA1208204 to W.M.), the National Natural Science Foundation of China (NSFC W2411049 to W.M., 52303246 to B.W., 523B2033 to S.W., 52503249 to S.W.), the China Postdoctoral Science Foundation (2022TQ0250 to B.W.), the Key Scientific and Technological Innovation Team Project of Shaanxi Province (2020TD-002 to W.M.), the Science and Technology Program of Shaanxi Province (2022JM-229 to W.M.), and the 111 Project 2.0 (BP2018008 to W.M.). China National Postdoctoral Program for Innovative Talents (BX20240282 to S.W.). J.N., N.S. and I.A. acknowledge financial support from the European Research Council (ERC) through the Advanced Grant (CAPaCITy, No. 742708). J.N. thanks the Royal Society for the award of a Research Professorship. The X-ray data were acquired at beamline 7.3.3 at the Advanced Light Source, which is supported by the Director, Office of Science, Office of Basic Energy Sciences, the U.S. Department of Energy under Contract No. DE-AC02-05CH11231.
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Zhang, S., Wang, B., Siemons, N. et al. Delayed cation dynamics enables dual-doped organic electrochemical transistors with high current sensitivity. Nat Commun (2026). https://doi.org/10.1038/s41467-026-73762-1
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DOI: https://doi.org/10.1038/s41467-026-73762-1
